Aqueous　nickel-zinc　(Ni-Zn)　batteries　hold　great　promise　for　large-scale　energy　storage　systems.　However,　traditional　Ni-based　cathode　electrodes　are　generally　consist　of　none　capacity　contribution　additives　and　heavy　current　collectors,　resulting　in　a　low　percentage　of　the　active　materials.　In　this　regard,　developing　lightweight,　flexible　and　binder-free　cathode　electrodes　for　aqueous　Ni-Zn　batteries　is　highly　desirable.　Herein,　for　the　first　time,　we　develop　a　simple　electrospinning　technique　to　synthesize　the　one-dimensional　(1D)　electrospun　carbon　nanofibers　functionalized　with　ternary　NiCo2S4　nanoparticles　(denoted　as　CNF@NiCo2S4)　as　a　lightweight,　flexible　and　binder-free　electrode　for　aqueous　Ni-Zn　batteries.　Based　on　the　self-standing　CNF@NiCo2S4　film　as　cathode,　the　as-fabricated　aqueous　CNF@NiCo2S4//Zn　battery　exhibits　a　high　capacity　of　0.32　mAh　cm−2　and　35.9　mAh　cm−3　at　a　current　density　of　2　mA　cm−2,　and　good　rate　performance　(0.21　mAh　cm−2　at　20　mA　cm−2)　and　long-term　cycling　stability　(83%　capacity　retention　at　10　mA　cm−2　after　2000　cycles).　More　importantly,　a　quasi-solid-state　CNF@NiCo2S4//Zn　battery　is　also　fabricated,　which　also　displays　an　impressive　energy　density　of　362.3　Wh　kg−1,　indicating　the　potential　towards　practical　applications.　Impressively,　the　volumetric　energy　density　of　CNF@NiCo2S4//Zn　battery　are　58.2　mWh　cm−3　(liquid)　and　45.4　mWh　cm−3　(quasi-solid-state),　which　are　much　larger　than　the　values　of　other　reported　Ni-Zn　batteries.　Theses　results　indicate　the　self-standing　CNF@NiCo2S4　film　is　promising　for　for　next　generation　electronic　applications.　©　2021